Review
Chemistry, Physical
Jiapian Huang, Zhiyuan Chen, Jie Wu
Summary: Methylation is a crucial process in biology, and radical-type methylation protocols have been developed for late-stage modifications of privileged scaffolds in pharmaceutical research. The chemistry involving methyl-radical-involved conversions has significantly developed in recent years. Various pathways for methyl radical generation have been explored, including photo-/electro-catalysis, transition-metal catalysis, transition-metal-free methylations, and demethylation-triggered radical cyclization/cascade reactions. Representative methyl-containing molecules produced from these reactions have been analyzed.
Article
Chemistry, Multidisciplinary
Tsz-Kan Ma, Diyuan Li, Jonathan D. Wilden
Summary: Mechanistic studies of a reactive oxygen species mediated electrochemical radical reaction of alkyl iodides are described. Hydroxyl radicals and ozone are identified as the active species involved in the formation of alkyl radicals under mildly reducing potential (-1.0 V vs. Ag QRE) in buffered acidic conditions (pH 3.6).
CHEMICAL COMMUNICATIONS
(2021)
Review
Biochemistry & Molecular Biology
Daniel Koch, Mohamed Chaker, Manabu Ihara, Sergei Manzhos
Summary: Density-driven descriptors are more suitable for characterizing the mechanism of redox reactions than formal oxidation states, especially when anion redox is involved. The description of redox reactions is critically important for understanding and rational design of materials for electrochemical technologies.
Article
Chemistry, Physical
Ralf Kaiser, Long Zhao, Wenchao Lu, Musahid Ahmed, Marsel Zagidullin, Valeriy N. Azyazov, Alexander M. Mebel
Summary: Resonantly stabilized free radicals are considered fundamental molecular building blocks in the formation of polycyclic aromatic hydrocarbons and carbonaceous nanoparticles. Research has shown the formation of benzene and naphthalene through specific reactions at elevated temperatures, providing important insights into organic hydrocarbon chemistry in high temperature circumstellar environments and combustion systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Medicinal
Junhui Lu, Huimin Zhang, Jinhui Yu, Dezun Shan, Ji Qi, Jiawen Chen, Hongwei Song, Minghui Yang
Summary: The study developed a machine learning approach to predict the temperature-dependent site-specific rate constants of hydrogen abstraction reactions, demonstrating robustness in accurately predicting the site-specific and overall rate constants.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2021)
Review
Chemistry, Organic
Saima Malik, Aditya G. Lavekar, Bimal Krishna Banik
Summary: Radical chemistry, which has a history of two centuries, focuses on radical-mediated reactions that attract organic chemists to prepare new compounds with diverse stereochemistry. The tin-based radical annulation method is commonly used for synthesizing a wide range of organic compounds with medicinal significance, following atom economical principles. Recent stereoselective tin-mediated radical cyclization reactions demonstrate the versatility of tin-based reagents in encouraging chemists to construct many other molecules of interest.
CURRENT ORGANIC CHEMISTRY
(2021)
Review
Chemistry, Multidisciplinary
Jose Aleman, Ruben Mas-Balleste
Summary: Covalent Organic Frameworks (COFs) and related extended organic materials have been widely utilized as photocatalysts, with the design process being influenced by factors like crystallinity and porosity. However, catalytic activity does not solely depend on these characteristics, as shown in a compilation of literature on the use of COFs and Covalent Triazine Frameworks (CTFs) in photocatalytic oxidation processes.
FRONTIERS IN CHEMISTRY
(2021)
Article
Chemistry, Physical
Andrew Hainer, Neeraj Joshi, Juan C. Scaiano
Summary: The chemistry resulting from the scavenging of hole in TiO2 can be easily observed using laser flash photolysis techniques. The transparent nature of dilute suspensions in the UV region allows for the monitoring of long-lived signals from reactions with solvent radicals. Transient signals from hole, electron, and trapped radicals exhibit stretched exponentials (nanoseconds to milliseconds) and can be well described by fractal models.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Review
Chemistry, Multidisciplinary
Nishitha Prakash, Rijo Rajeev, Anjali John, Ajesh Vijayan, Louis George, Anitha Varghese
Summary: The interest in green and sustainable chemistry has led to the development of different synthetic methods utilizing clean reagents, with electro-oxidation reactions being considered one of the most promising methods. TEMPO, a stable aminoxyl radical, is commonly used for the oxidation of alcohols to carbonyl compounds. The review discusses various electrochemical reactions using TEMPO as a mediator and provides a basis for future studies on better electrocatalyst design involving TEMPO and its derivatives.
Article
Chemistry, Physical
Wanyi Liao, Qin Zhao, Shanshan Wang, Yiling Ran, Hong Su, Rong Gan, Shun Lu, Yan Zhang
Summary: The high energy consumption in water electrolysis systems is attributed to the slow kinetics of the oxygen evolution reaction (OER). Substituting thermodynamically advantageous small molecule oxidation reactions for OER can significantly improve energy conversion efficiency. Studying the in-depth reaction mechanism of complex substrates is necessary due to their elemental composition. This review focuses on the electrooxidation mechanism of different substrate molecules, such as ethanol, urea, and hydrazine, and introduces design ideas and strategies for high-performance electrocatalysts in relation to reaction path selectivity. The challenges in achieving industrial transformation in this field are also discussed.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
Roel F. J. Epping, David Vesseur, Minghui Zhou, Bas de Bruin
Summary: Discovered in the 1970s as organometallic curiosities, carbene radicals have become essential in modern homogeneous catalysis. These radicals exhibit nucleophilic reactivity different from electrophilic Fischer carbenes. The successful catalytic application of carbene radicals has led to the synthesis of diverse carbon and heterocyclic compounds. This Perspective provides an overview of the coordination chemistry, reactivity, and catalytic application of carbene radicals using transition metal complexes and catalysts since 2011.
Article
Chemistry, Multidisciplinary
Cai-Wu Luo, Lei Cai, Chao Xie, Gang Li, Tian-Jiao Jiang
Summary: The presence of sulfur vacancies in MoS2 catalysts enhances their catalytic activity in Fenton-like reactions for the removal of organic pollutants in wastewater. The annealing temperature and pH value significantly influence the performance of the catalysts. The reaction system contains both radical and non-radical species.
Review
Chemistry, Multidisciplinary
Lianping Wu, Teng Li
Summary: Atomic catalysts (ACs) have shown great potential as high-performance catalysts due to their ultimate atomic utilization and unique catalytic properties. However, their rational design is cost-prohibitive, and machine learning (ML) has emerged as a promising approach to accelerate the study of ACs and screen high-performance catalysts efficiently. This review highlights recent advances in the ML-enabled rational design of ACs, focusing on the efficient selection of high-performance ACs for various electrochemical reactions.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Review
Chemistry, Organic
Pooja Yadav, A. Anagha Varma, A. J. Punnya, Purushothaman Gopinath
Summary: Multicomponent reactions (MCR's) offer synthetic chemists the opportunity to synthesize complex organic molecules in a single step, but their applications are limited by control difficulties of desired reactivity and selectivity with three or more components. Photoredox catalysis has gained attention from synthetic chemists for its simplicity and new reactivity. A review of existing reports is essential for the further design of photomediated multicomponent reactions.
ASIAN JOURNAL OF ORGANIC CHEMISTRY
(2022)
Review
Biochemistry & Molecular Biology
Tomasz Bauer, Yusuf Zaim Hakim, Paulina Morawska
Summary: This review covers recent research on enantioselective synthesis using radical reactions, focusing on the synthesis of chiral molecules through metal catalysis, dual metal and organocatalysis, and pure organocatalysis including enzyme catalysis. The review highlights the synthetic aspects of the methodology and discusses the compounds that can be obtained in enantiomerically enriched forms.
Article
Chemistry, Physical
A. S. Rasal, Y-H Chen, K. Dehvari, G. Getachew, P-J Tseng, K. Waki, S. Bela, J-Y Chang
Summary: This study reported the preparation of a gel electrolyte using XG and TiO2 NPs to improve the performance of QDSSCs, achieving higher photoconversion efficiencies and stability. XG exhibited thixotropic sol-gel transitions, and the incorporation of TiO2 NPs improved the ionic conductivity of the gel electrolyte, passivating surface trap states or acting as steric hindrance.
MATERIALS TODAY ENERGY
(2021)
Article
Nanoscience & Nanotechnology
Girum Getachew, Chiranjeevi Korupalli, Akash S. Rasal, Worku Batu Dirersa, Mochamad Z. Fahmi, Jia-Yaw Chang
Summary: For the first time, red-emitting CsMgxPb1-xI3 quantum dots were prepared by doping with magnesium ions, showing excellent optical properties and outstanding biocompatibility. By encapsulating into PF127-Gd micelles, the bioavailability of the quantum dots was improved. Overall, this study proposes a novel strategy to enhance the optical properties, stability, and bioapplicability of quantum dots.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Engineering, Biomedical
Novi Irmania, Khalilalrahman Dehvari, Jia-Yaw Chang
Summary: In this study, a new set of multifunctional chalcogenide quantum dots was synthesized via a one-pot microwave-assisted hydrothermal reaction, and their potential applications in dual-modal imaging and therapy were demonstrated.
JOURNAL OF BIOMATERIALS APPLICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Akash S. Rasal, Ting-Ying Lee, Pei-Yun Kao, Girum Gatechew, Aswandi Wibrianto, Worku Batu Dirersa, Anil Ghule, Jia-Yaw Chang
Summary: In this study, a simple and direct approach was used to develop high-quality counter electrode films for quantum dot-sensitized solar cells. By combining metallic copper chalcogenides with S, N dual-doped carbon sources, the resulting films demonstrated improved photovoltaic performance.
Article
Chemistry, Multidisciplinary
W. B. Dirersa, G. Getachew, C. -H Hsiao, A. Wibrianto, A. S. Rasal, C. -C. Huang, J. -Y. Chang
Summary: This study reported the ROS-mediated therapies of CuFeS2 nanoparticles, which showed good efficacy in photothermal, photodynamic, and chemodynamic therapies. Furthermore, the nanoparticles were used for drug delivery to enhance chemotherapy. The results demonstrated the potential of these nanoparticles as anticancer agents.
MATERIALS TODAY CHEMISTRY
(2022)
Article
Chemistry, Physical
Aswandi Wibrianto, Girum Getachew, Worku Batu Dirersa, Akash S. Rasal, Chih-Ching Huang, Tzu-Chun Kan, Jungshan Chang, Jia-Yaw Chang
Summary: Clinical studies have shifted to multimodal therapy due to the complexity and unpredictability of malignant tumors. This study presents a one-pot microwave synthesis of highly fluorescent copper, nitrogen, and sulfur-doped carbon quantum dots (Cu,N,S-CQDs) with superior quantum yield and enhanced peroxidase-like activity. These Cu,N,S-CQDs were further biofunctionalized with glucose oxidase (GOx) and camptothecin (CPT) to form a multifunctional nanocatalyst for cancer therapy. The Cu,N,S-CQDs@GOx/CPT nanocatalyst demonstrated multiple therapeutic mechanisms, including chemodynamic therapy, gas therapy, starvation therapy, and chemotherapeutic mechanisms.
Article
Energy & Fuels
Rutuja A. Chavan, Gokul P. Kamble, Sarika B. Dhavale, Akash S. Rasal, Sanjay S. Kolekar, Jia-Yaw Chang, Anil Vithal Ghule
Summary: MXene composites with different metal oxides have shown good electrochemical performance and hinder restacking of MXene. In this study, nickel oxide@MXene (NO@MXene) composites with varying compositions were synthesized and used as an anode for a supercapacitor. The 15% NO@MXene composite electrode demonstrated the highest capacitance, and an all-solid-state asymmetric supercapacitor with 15% NO@MXene as the anode displayed good cyclic stability and high energy and power densities.
Article
Chemistry, Multidisciplinary
Yao-Sheng Cheng, Yu-Ting Wu, Sofiannisa Aulia, Ching-Cheng Chang, Mia Rinawati, Ting-Ying Lee, Jia-Yaw Chang, Ni Luh Wulan Septiani, Brian Yuliarto, Min-Hsin Yeh
Summary: A quantum dot-sensitized solar cell (QDSSC) with cobalt manganese sulfide (CMS) composites as counter electrodes (CE) exhibits improved activity and stability. By controlling the precursor ratio of Co and Mn, the bimetallic CMS can be adjusted to manipulate the Sn2- reduction activity. The optimized CMS CEs also demonstrate a high solar-to-electricity conversion efficiency of 5.88 +/- 0.19% under 100 mW cm-2 irradiation, indicating their superior reduction activity to Sn2-.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Materials Science, Multidisciplinary
Livy Laysandra, Girum Getachew, Jai-Rui Chang, Jia-Yaw Chang, Yu-Cheng Chiu
Summary: Achieving polymer nanocomposites with improved elasticity and stable mechanical and fluorescence properties remains challenging. However, the grafting from method coupled with reversible fragment-added chain transfer polymerization shows promise for the preparation of flexible and fluorescent nanocomposite films.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Chemistry, Physical
Worku Batu Dirersa, Girum Getachew, Aswandi Wibrianto, Akash S. Rasal, Vivek S. Gurav, Mochamad Zakki Fahmi, Jia-Yaw Chang
Summary: The development of multifunctional nano-therapies has improved cancer treatment by enhancing therapeutic performance and minimizing side effects. In this study, a drug-loaded nanocarrier was designed for multimodal cancer therapy using MoOxS2-x quantum dots. The nanocarrier demonstrated efficient catalytic activity for chemodynamic treatment, reactive oxygen species-mediated therapies, and photodynamic therapy. It also exhibited excellent drug-loading efficiency and biocompatibility, resulting in significant cancer cell death through various therapeutic mechanisms.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Polymer Science
Tzu-Chi Chiang, Jia-Yaw Chang, Tzung-Han Chou
Summary: This study successfully prepared stable nanoemulsions of curcumin by adjusting the HLBt using Tween 60. The addition of Tween 60 reduced the size of the nanoemulsions and improved their storage stability. Higher HLBt values resulted in higher encapsulation efficiency and enhanced remaining activity of curcumin.
Article
Nanoscience & Nanotechnology
Worku Batu Dirersa, Tzu-Chun Kan, Girum Getachew, Aswandi Wibrianto, Sonjid Ochirbat, Akash Rasal, Jungshan Chang, Jia-Yaw Chang
Summary: Iron-containing Fenton nanocatalysts have shown great potential for clinical use due to their effective antitumor activity and low toxicity. In this study, FeMnOx nanoparticles were synthesized using cation exchange to enhance Fenton reactions in the tumor microenvironment, leading to improved chemodynamic therapy and chemotherapy. The nanoparticles exhibited excellent therapeutic potential, as demonstrated in in vitro and animal studies.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Review
Materials Science, Multidisciplinary
Girum Getachew, Aswandi Wibrianto, Akash S. Rasal, Shamsa Kizhepat, Worku Batu Dirersa, Vivek Gurav, Jia-Yaw Chang
Summary: This article presents an in-depth investigation of lead-free perovskite material quantum dots (LFPMs QDs) as photocatalysts. LFPMs show promising performance in various photocatalysis applications, including water splitting, CO2 reduction, pollutant degradation, and organic synthesis. The formation of heterojunction nanocomposites using LFPMs and co-catalysts or hole-transporting materials enhances their photocatalytic performance. The article also discusses the advantages and drawbacks of LFPMs photocatalysts and proposes future research directions.
PROGRESS IN MATERIALS SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Wulan Purnamasari, Titah Aldila Budiastanti, Aminatun Aminatun, Ulfa Rahmah, Sri Sumarsih, Jia-Yaw Chang, Mochamad Zakki Fahmi
Summary: The present study investigated the effect of graphene oxide in cellulose acetate-based composite nanofibers on the transdermal delivery of naproxen. The addition of graphene oxide promoted the production of nanofibers with smaller diameter, higher conductivity, and higher mechanical strength, resulting in higher naproxen release from the nanofibers. The composite nanofiber also exhibited antibacterial activity and accelerated naproxen release at neutral pH, showing potential for wound healing applications.
Article
Nanoscience & Nanotechnology
Girum Getachew, Chiranjeevi Korupalli, Akash S. Rasal, Worku Batu Dirersa, Mochamad Z. Fahmi, Jia-Yaw Chang
Summary: This study reports the preparation of red-emitting CsMgxPb1-xI3 quantum dots (QDs) and their biofunctionalization into gadolinium-conjugated pluronic 127 micelles (PQD@Gd) for dual-modal imaging and photodynamic therapeutic properties. The PQD@Gd nanoagents exhibit superior MR contrasting effects and have potential applications in cancer therapy and organic pollutant removal. Additionally, the PQD@Gd nanoagents demonstrate excellent photocatalytic activity towards organic pollutants under visible light irradiation, showcasing their multifunctionality.
ACS APPLIED MATERIALS & INTERFACES
(2022)